期刊
SCIENCE
卷 329, 期 5987, 页码 65-69出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1189588
关键词
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资金
- NSF [CHE-0908548]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0908548] Funding Source: National Science Foundation
Since the discovery of the hydrated electron more than 40 years ago, a general consensus has emerged that the hydrated electron occupies a quasispherical cavity in liquid water. We simulated the electronic structure and dynamics of the hydrated electron using a rigorously derived pseudopotential to treat the electron-water interaction, which incorporates attractive oxygen and repulsive hydrogen features that have not been included in previous pseudopotentials. What emerged was a hydrated electron that did not reside in a cavity but instead occupied a similar to 1-nanometer-diameter region of enhanced water density. Both the calculated ground-state absorption spectrum and the excited-state spectral dynamics after simulated photoexcitation of this noncavity hydrated electron showed excellent agreement with experiment. The relaxation pathway involves a rapid internal conversion followed by slow ground-state cooling, the opposite of the mechanism implicated by simulations in which the hydrated electron occupies a cavity.
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